The invention discloses a method for removing carbons in polysilicon carbon head materials, which mainly comprises the following steps: crushing carbon head materials, then separating the obtained products into three categories, wherein the three categories of materials are as follows: the category-one materials are carbon-free silicon blocks which are unnecessary to be cleaned, the category-two materials are silicon blocks with a carbon layer (thickness: less than 1cm) on the surface thereof, and the category-three materials are silicon blocks sandwiched with a carbon layer or provided with a carbon layer (thickness: greater than 1cm) on the surface thereof; the category-two materials and the category-three materials are required to be cleaned by different carbon-silicon separating solutions, then sequentially performed with water scrubbing, purging, pickling, water scrubbing and drying, wherein the carbon-silicon separating solution of the category-two materials is a mixed solution of concentrated sulfuric acids, concentrated nitric acids and potassium permanganates, and the carbon-silicon separating solution of the category-three materials is a mixed solution of concentrated sulfuric acids and potassium permanganates. The method of the invention is implemented through starting with the process of separating carbon head materials, and different materials are processed by using different methods, thereby improving the efficiency and reducing the cost.